US7037472B2 - Single-pipe cylinder-type reformer - Google Patents

Single-pipe cylinder-type reformer Download PDF

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US7037472B2
US7037472B2 US09/969,718 US96971801A US7037472B2 US 7037472 B2 US7037472 B2 US 7037472B2 US 96971801 A US96971801 A US 96971801A US 7037472 B2 US7037472 B2 US 7037472B2
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flow path
gas flow
path section
gas
section
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US20020042035A1 (en
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Jun Komiya
Toshiyasu Miura
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Tokyo Gas Co Ltd
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Tokyo Gas Co Ltd
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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/06—Combination of fuel cells with means for production of reactants or for treatment of residues
    • H01M8/0606—Combination of fuel cells with means for production of reactants or for treatment of residues with means for production of gaseous reactants
    • H01M8/0612—Combination of fuel cells with means for production of reactants or for treatment of residues with means for production of gaseous reactants from carbon-containing material
    • H01M8/0625—Combination of fuel cells with means for production of reactants or for treatment of residues with means for production of gaseous reactants from carbon-containing material in a modular combined reactor/fuel cell structure
    • H01M8/0631—Reactor construction specially adapted for combination reactor/fuel cell
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    • B01J8/02—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds
    • B01J8/04—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds the fluid passing successively through two or more beds
    • B01J8/0446—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds the fluid passing successively through two or more beds the flow within the beds being predominantly vertical
    • B01J8/0461—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds the fluid passing successively through two or more beds the flow within the beds being predominantly vertical in two or more cylindrical annular shaped beds
    • B01J8/0465—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds the fluid passing successively through two or more beds the flow within the beds being predominantly vertical in two or more cylindrical annular shaped beds the beds being concentric
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    • C01B3/38—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents using catalysts
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    • C01B3/48—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents followed by reaction of water vapour with carbon monoxide
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    • B01J2208/00008—Controlling the process
    • B01J2208/00017—Controlling the temperature
    • B01J2208/00504—Controlling the temperature by means of a burner
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    • C01B2203/0205—Processes for making hydrogen or synthesis gas containing a reforming step
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    • C01B2203/0844—Methods of heating the process for making hydrogen or synthesis gas by heat exchange with exothermic reactions, other than by combustion of fuel the non-combustive exothermic reaction being another reforming reaction as defined in groups C01B2203/02 - C01B2203/0294
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Definitions

  • the present invention relates to a single-pipe cylinder-type reformer for manufacturing a hydrogen-rich reformed gas by steam-reforming a hydrocarbon-based fuel such as a city gas or LPG and, more particularly, to a reformer used in a solid-state polymer-type fuel cell.
  • a reformer is an apparatus for generating a reformed gas with a high hydrogen concentration by steam-reforming a raw material gas such as a city gas or LPG, and is widely used when manufacturing hydrogen used in an optical fiber or semiconductor manufacturing process, a fuel cell and the like.
  • the steam-reforming reaction performed by a reformer is an endothermic reaction, and accordingly heating is needed to sustain the reaction.
  • a combustor such as a burner is added to the reformer, and excessive hydrogen or reformed raw material gas from a fuel cell is heated by combusting it with the burner.
  • a reformer for manufacturing a comparatively small volume of hydrogen for example, a single-pipe cylinder-type reformer as disclosed in Japanese Unexamined Patent Publication No. 11-11901 is known.
  • a heating means such as a burner is provided at the center of a cylindrical container comprised of two cylinders with a catalyst layer being stored between them. The catalyst layer is heated by the heating means, and a raw material gas supplied to the catalyst layer is reformed by steam.
  • the entire reforming device including the single-pipe cylinder-type reformer must be made compact and lightweight. Also, various types of improvements must be made; e.g. higher-efficiency operation must be realized and the start-up time at the start of operation must be shortened.
  • the raw material gas must be efficiently pre-heated to reduce the fuel.
  • Overheating of the steam generator must be prevented to make the reformer more convenient to use.
  • the reformer must be held at the necessary temperature and the quantity of heat must be effectively utilized to improve efficiency.
  • External heat dissipation must be suppressed by an effective heat insulating structure.
  • Thermal stress caused by an internal temperature difference must be moderated to realize a high durability.
  • the heat of reaction must be effectively utilized to generate steam efficiently.
  • the reformed gas generated by the conventional single-pipe cylinder-type reformer contains about 10% of CO.
  • the CO concentration must be decreased to about 0.5% by a CO modifier, and CO selective oxidation must be performed by a CO selective oxidizer, so the CO concentration decreases to about 10 ppm.
  • providing a CO modifier and a CO selective oxidizer for this purpose independently of the single-pipe cylinder-type reformer is not preferable in terms of downsizing, high efficiency, and start-up performance.
  • the present invention has been made in consideration of the above problems in the prior art, has as an object to provide a single-pipe cylinder-type reformer which can generate a reformed gas with a low CO concentration, has an efficient, good start-up performance, realizes reduction in size and weight and does not emit excessive heat.
  • a single-pipe cylinder-type reformer including a plurality of circular cylinders standing upright coaxially and forming therebetween a gas flow path allowing a raw material gas to flow therein and having a plurality of gas flow path sections, each being disposed between every pair of adjacent circular cylinders and having an annular cross-section, a radiation cylinder coaxially arranged inside the plurality of circular cylinders and forming at an outer periphery thereof an exhaust flow path, a burner arranged at one end of a center of the radiation cylinder for generating a combustion gas allowed to flow within the exhaust flow path in the reverse direction to the flowing direction of the raw material gas in a first gas flow path section, a reforming catalyst layer obtained by packing with a reforming catalyst into at least the first gas flow path section closest to the burner among the plurality of gas flow path sections, in which the raw material gas is reformed by making use of only steam, comprising a metal pre-heat
  • a single-pipe cylinder-type reformer including a plurality of circular cylinders standing upright coaxially and forming therebetween a gas flow path allowing a raw material gas to flow therein and having a plurality of gas flow path sections, each being disposed between every pair of adjacent circular cylinders and having an annular cross-section, a radiation cylinder coaxially arranged inside the plurality of circular cylinders and forming at an outer periphery thereof an exhaust flow path, a burner arranged at one end of a center of the radiation cylinder for generating a combustion gas allowed to flow within the exhaust flow path in the reverse direction to the flowing direction of the raw material gas in a first gas flow path section, a reforming catalyst layer obtained by packing with a reforming catalyst into at least the first gas flow path section closest to the burner among the plurality of gas flow path sections, in which the raw material gas is reformed by making use of only steam, comprising a metal pre-heat
  • a single-pipe cylinder-type reformer according to the first and second aspects described above, further comprising a second gas flow path section with an annular cross-section, the second gas flow path section being formed outside the reforming catalyst layer packed with the reforming catalyst, communicating with the reforming catalyst layer with one end-side inlet port thereof, and allowing a gas to flow in a direction opposite to that of a gas flow in the first gas flow path section, wherein the other end-side outlet port of the second gas flow path section is arranged on an outer peripheral side near an inlet port of the pre-heat layer, and helical dividing means extending in an axial direction of the circular cylinders is formed in the second gas flow path section, for helically dividing a gas and making it flow through the second gas flow path section.
  • a single-pipe cylinder-type reformer according to the first or second aspect described above, further comprising
  • the second gas flow path section being formed around the reforming catalyst layer packed with the reforming catalyst, communicating with the reforming catalyst layer with one end-side inlet port thereof, and allowing a gas to flow in a direction opposite to that of a gas flow in the first gas flow path section,
  • a third gas flow path section with an annular cross-section, the third gas flow path section being formed around the second gas flow path section, communicating with the other end-side outlet port of the second gas flow path section with one end-side inlet port thereof, allowing a gas to flow in a direction opposite to that of a gas flow in the second gas flow path section, and being provided with dividing means and a CO modifying catalyst layer therein,
  • a fourth gas flow path section with an annular cross-section, the fourth gas flow path section being formed around the third gas flow path section, communicating with the other end-side outlet port of the third gas flow path section with one end-side inlet port thereof, allowing a gas to flow in a direction opposite to that of a gas flow in the third gas flow path section, and being provided with a CO selective oxidation catalyst layer therein, and
  • a heating channel which serves as a raw material gas flow path section formed between the third and fourth gas flow path sections, has an inlet port at one end side thereof, and allows a raw material gas in the fourth gas flow path section to flow in a direction opposite to that of a gas flow in the fourth gas flow path section and to reverse near one end of the fourth gas flow path section, and allows the raw material gas in the third gas flow path section to flow in the same direction as that of a gas flow in the fourth gas flow path section.
  • a single-pipe cylinder-type reformer according to the first or second aspect described above, further comprising
  • the second gas flow path section being formed around the reforming catalyst layer packed with the reforming catalyst, communicating with the reforming catalyst layer with one end-side inlet port thereof, and allowing a gas to flow in a direction opposite to that of a gas flow in the first gas flow path section,
  • a third gas flow path section with an annular cross-section, the third gas flow path section being formed around the second gas flow path section, communicating with the other end-side outlet port of the second gas flow path section with one end-side inlet port thereof, allowing a gas to flow in a direction opposite to that of a gas flow in the second gas flow path section, and being provided with a CO modifying catalyst layer therein,
  • a fourth gas flow path section with an annular cross-section, the fourth gas flow path section being formed around the third gas flow path section, communicating with the other end-side outlet port of the third gas flow path section with one end-side inlet port thereof, allowing a gas to flow in a direction opposite to that of a gas flow in the third gas flow path section, and being provided with a CO selective oxidation catalyst layer therein,
  • a heating channel which serves as a raw material gas flow path section formed between the third and fourth gas flow path sections, has an inlet port at one end side thereof, and allows a raw material gas in the fourth gas flow path section to flow in a direction opposite to that of a gas flow in the fourth gas flow path section and to reverse near one end of the fourth gas flow path section, and allows the raw material gas in the third gas flow path section to flow in the same direction as that of a gas flow in the fourth gas flow path section,
  • annular mixing chamber to be connected to an air supply pipe on an upstream side of the fourth gas flow path section
  • axial lengths of the third and fourth gas flow path sections are shorter than those of the first and second gas flow path sections, and a second CO modifying catalyst layer is formed on an upstream side of the fourth gas flow path section.
  • the present invention has the following several auxiliary aspects.
  • Helical dividing means extending in an axial direction of the circular cylinders is provided in the pre-heat layer and the reforming catalyst layer so that a gas helically flows through the first gas flow path section.
  • the helical dividing means is comprised of a plurality of helical fins or a plurality of helical round rods that divide the gas flow path sections into sectors in cross-sections thereof.
  • the dividing means formed in the second gas flow path section is comprised of a plurality of round rods that divide the second gas flow path section into sectors in a cross-section thereof.
  • the dividing means formed in the third gas flow path section is comprised of a plurality of fins fixed to an inner circular cylinder that forms the third gas flow path section, so as to divide the third gas flow path section into sectors in a cross-section thereof.
  • An outer circumferential wall of the CO selective oxidation catalyst layer is formed inside an outer circumferential wall of the fourth gas flow path section, and a space formed between the outer circumferential wall of the fourth gas flow path section and the outer circumferential wall of the CO selective oxidation catalyst layer and divided from the mixing chamber serves as a cooling flow path where a cooling fluid flows.
  • a dividing member is provided in the cooling flow path to divide the cooling flow path helically.
  • the cooling fluid to be supplied into the cooling flow path is supplied to flow in a direction opposite to a flowing direction of a gas to be supplied into the CO selective oxidation catalyst layer.
  • Combustion air to be combusted by the burner or an OFF gas discharged from a fuel pole of a fuel cell is used as the cooling fluid.
  • the pre-heat layer having the packing is formed in the preceding step to the reforming catalyst layer, a raw material pre-heater becomes unnecessary, agitation can be performed efficiently, and the quantity of heat consumption can be decreased.
  • the inlet port of the pre-heat layer and the outlet port of the second gas flow path section are close to each other, the temperature of the outlet port of the second gas flow path section can be decreased, and the reforming catalyst layer and the CO modifying catalyst layer can be directly connected.
  • the interiors of the pre-heat layer, reforming catalyst layer, and other gas flow path sections are helically formed by fins or the like, a uniform temperature distribution can be obtained and the heat recovery efficiency can be improved, so the temperature of the outlet port can be set to a desired value.
  • the reformer can be integrally formed to include the CO selective oxidation catalyst layer. Since the reaction heat of the CO modifying catalyst layer and CO selective oxidation catalyst layer can be recovered, the efficiency can be improved. Also, an undesirable side reaction can be suppressed.
  • the wall surface of the second gas flow path section and that of the CO modifying catalyst layer are formed separately and a gap is formed between them, heat insulation between these wall surfaces is improved, the recovery efficiency in the flow path section is improved, temperature increase of the CO modifying catalyst layer can be suppressed, and any heat stress acting between these wall surfaces can be avoided.
  • Gas and air can be uniformly mixed in the mixing chamber, so a hydrogen loss can be decreased.
  • the reforming water can be evaporated by the heating channel formed between the CO modifying catalyst layer and CO selective oxidation catalyst layer, a boiler can be formed without using a fuel. Also, a sufficiently high cooling ability for the CO modifying catalyst layer and CO selective oxidation catalyst layer can be obtained.
  • the reformer can be used as a hydrogen generator for a solid-state polymer-type fuel cell, thus forming a compact, highly efficient fuel cell.
  • the gas flow path section formed of the CO modifying catalyst layer and CO selective oxidation catalyst layer is shortened to be shorter than an opposing gas flow path section, excessive temperature increase of the CO modifying catalyst layer can be prevented. Since the CO modifying catalyst layer is held at an appropriate temperature, the reaction is not interfered with.
  • the temperature of the CO modifying catalyst layer can be increased quickly, the reaction of the CO modifying catalyst layer can be performed immediately after operation is started, and the start-up operation of the reformer can be quickened.
  • FIG. 1 is a longitudinal sectional view showing the schematic arrangement of a single-pipe cylinder-type reformer according to an embodiment of the present invention
  • FIG. 2 is a partial cross-sectional view of the single-pipe cylinder-type reformer according to the embodiment of the present invention.
  • FIG. 3 is a partial side view of the single-pipe cylinder-type reformer according to the embodiment of the present invention.
  • FIG. 1 shows the schematic arrangement of a single-pipe cylinder-type reformer.
  • a single-pipe cylinder-type reformer the respective cylinders of which stand vertically and the burner of which is attached to one end (an upper portion in FIG. 1 ) of the reformer, as shown in FIG. 1 , will be described as an example.
  • a reformer 2 is constituted by a plurality of circular cylinders 6 comprised of first to ninth cylinders 61 to 69 mounted coaxially, ring-shaped gaps defined between the respective cylinders, which forms a zigzag gas flow path having a plurality of gas flow path sections disposed between every pair of adjacent circular cylinders, a burner 18 mounted on the side of one end of the first cylinder 61 and at the center thereof, a reforming catalyst layer 8 , CO modifying catalyst layer 10 (to be referred to also as a shift layer 10 hereinafter), and CO selective oxidation catalyst layer 12 ( 13 )(to be referred to also as a PROX layer 12 ( 13 ) hereinafter) arranged in spaces formed by the respective cylinders and the like.
  • the reformer 2 has a water supply port 20 , a combusted exhaust gas outlet port 24 , a raw material gas supply port 26 , a reformed gas outlet port 28 , and PROX air supply ports 30 and 32 in its side surface.
  • a cylindrical heat transfer partition wall 14 (radiation cylinder) is arranged inside the first cylinder 61 to be coaxial with it while leaving an appropriate gap around and under the partition wall 14 . This gap serves as an exhaust flow path 80 .
  • the exhaust flow path 80 is connected at its upper portion to the combusted exhaust gas outlet port 24 so that the exhaust gas combusted by the burner 18 is allowed to flow to thereby be exhausted from the combusted exhaust gas outlet port 24 .
  • the burner 18 is attached inside the heat transfer partition wall 14 through a burner base 16 .
  • a water heating channel 34 communicating with the water supply port 20 is formed between the exhaust flow path 80 and burner base 16 .
  • the water heating channel 34 is connected to a raw material gas supply path 27 through a connecting pipe 25 formed at a position opposing the supply port 20 , and the supply path 27 is connected to the raw material gas supply port 26 .
  • a first gas flow path section 51 with a predetermined width is formed between the first and second cylinders 61 and 62 .
  • a portion above the first gas flow path section 51 is a pre-heat layer 51 a
  • a portion under the pre-heat layer 51 a is the reforming catalyst layer 8 .
  • Four heat transfer fins 9 are provided between the first and second cylinders 61 and 62 to extend radially from the first cylinder 61 toward the second cylinder 62 , so as to helically surround substantially the entire circumference of the first cylinder 61 , as shown in FIG. 3 .
  • the four fins 9 helically divide the first gas flow path section 51 between the first and second cylinders 61 and 62 .
  • FIG. 2 shows a cross-sectional view.
  • the helical fins 9 need not surround the entire circumference of the first cylinder 61 .
  • the number of fins 9 is not limited to four, but can be between about one and twenty.
  • the pre-heat layer 51 a communicates at its upper portion with a heating channel 48 connected to the raw material gas supply path 27 .
  • a raw material gas and water (steam or the like) flow into the pre-heat layer 51 a through the heating channel 48 .
  • the pre-heat layer 51 a is packed with a metal packing with a high heat transfer coefficient and predetermined shape.
  • the pre-heat layer 51 a heats them.
  • the fins 9 transfer the heat of the exhaust flow path 80 to the pre-heat layer 51 a and swirl the gas flow in the pre-heat layer 51 a so as to mix the gas efficiently.
  • the metal packing that is packed in the pre-heat layer 51 a will be described briefly.
  • the metal packing has a heat transfer performance about ten times larger than that of the ceramic balls.
  • the heat transfer area can accordingly be decreased, so that a fuel processor such as a reformer can be downsized.
  • the agitating effect may be increased in addition to the heat transfer performance.
  • the more the heat gas flowing in the pre-heat chamber causes a turbulent flow the higher the heat transfer effect becomes.
  • the shape of the packing to be packed in the pre-heat layer 51 a varies, e.g. a saddle shape, a macaroni-like shape, and a mesh-like shape, in addition to a basic spherical shape. While the manufacturable shape of the ceramic packing is limited due to the strength, if a metal packing the shape of which is controllable is employed, a shape which has a larger surface area and can cause a turbulent flow more easily than the ceramic packing with the same area does can be obtained easily.
  • a large surface area can mean a large void (a space not occupied by a bulk such as a metal).
  • the weight can be decreased accordingly, and the heat capacity of the packing can be decreased. If the heat capacity is small, the time required for heating the packing at the start-up of the reformer shortens, so the start-up performance is improved.
  • the void is 85% to 98% on the higher side, and the void of the packing used in the present invention is 96.8%.
  • the void of the ceramic packing such as an alumina packing is about 60% to 70%.
  • the only drawback of the metal packing is that its material is rather expensive. Increasing the cost of material in a large plant that basically operates continuously when the metal packing is to be used is an issue, because it is less important for the large plant to improve a capability for dealing with set-up operation and load variation thereof.
  • the reformer of the present invention is a home-use plant of about 1 kWe class. Therefore, it is necessary to perform a set-up/stop operation of the reformer one or two times a day, and further it is very important to improve the capability for dealing with load variation in accordance with a demand for electric power. Thus, it is very effective to adopt the material of the metal packing.
  • the reforming catalyst layer 8 is packed with a reforming catalyst for steam-reforming the raw material gas.
  • the first gas flow path section 51 formed with the reforming catalyst layer 8 opens, at the lower portion of the reformer 2 , to a space formed between a bottom plate 71 of the first cylinder 61 and a bottom plate 73 of the third cylinder 63 .
  • the gap between the bottom plates 71 and 73 is formed so as to allow a stress generated at the time when the cylinders 61 , 62 and 63 are respectively elongated by heat. Further, it also serves as a heat-insulating layer against the flame of the burner 18 .
  • the fins 9 are provided to the first gas flow path section 51 formed with the reforming catalyst layer 8 , as described above.
  • the heat of the exhaust flow path 80 is transferred to the interior of the reforming catalyst layer 8 . Because of the flow paths helically formed by the fins 9 , the temperature difference is small, so that a reforming reaction occurs efficiently.
  • a second gas flow path section 50 with a predetermined width is formed between the second and third cylinders 62 and 63 , and is helically divided by four round rods 81 .
  • a gap is formed between the third and fourth cylinders 63 and 64 .
  • An insulator 53 is packed in this gap to reduce heat transfer.
  • a third gas flow path section 52 with a predetermined width is formed between the fourth and fifth cylinders 64 and 65 .
  • the shift layer CO(CO modifying catalyst layer) 10 packed with a Co modifying catalyst is formed in the third gas flow path section 52 .
  • a CO modifying reaction takes place in the shift layer 10 .
  • sixteen fins 11 are formed in the shift layer 10 to be parallel to the axial direction. Each fin 11 is fixed to the fourth cylinder 64 and is directed to the fifth cylinder 65 with its other end, so that the internal temperature of the shift layer 10 is uniform. Alternatively, the fins 11 may be formed helically to form helical flow paths, and the number of fins 11 is not limited to sixteen.
  • the upper portion of the shift layer 10 communicates with the second gas flow path section 50 , and the lower portion thereof communicates with the first PROX layer (CO selective oxidation catalyst layer) 12 formed between the seventh and eighth cylinders 67 and 68 .
  • the first PROX layer 12 is packed with a CO selective oxidation catalyst, and causes an oxidation reaction that decreases the CO content to the order of ppm.
  • the fourth cylinder 64 is connected at its lower portion to the bottom of the ninth cylinder 69 .
  • a heating channel 48 with the sixth cylinder 66 therein is formed between the fifth and seventh cylinders 65 and 67 .
  • the raw material gas supplied from the raw material gas supply port 26 and water supplied from the water supply port 20 are heated when passing through the heating channel 48 , and are sent to the pre-heat layer 51 a .
  • Four round rods 82 are formed spatially helically in the outer flow path of the heating channel 48 , to divide the flow paths such that they extend helically to surround substantially the entire circumference of the heating channel 48 .
  • the first PROX layer 12 , a second PROX layer 13 , first and second mixing chambers 42 and 46 for mixing the gas and air and supplying the mixture to the first and second PROX layers 12 and 13 and the like are formed between the seventh and ninth cylinders 67 and 69 .
  • the shift layer 10 is formed, under a screen 31 , in the lower portion of the space between the seventh and ninth cylinders 67 and 69 .
  • Eight discharge ports 33 are formed in the screen 31 in the circumferential direction and communicate with the first mixing chamber 42 .
  • the first mixing chamber 42 is connected to the first air supply port 32 . Air is supplied to the first mixing chamber 42 through the first air supply port 32 and is mixed with the gas from the shift layer 10 .
  • the first mixing chamber 42 communicates with a chamber 44 , formed between the seventh and eighth cylinders 67 and 68 , through one inlet port 35 formed in the side surface of the eighth cylinder 68 .
  • the chamber 44 is formed outside the seventh cylinder 67 in the circumferential direction, and communicates with the first PROX layer 12 through eight inflow ports 37 formed in a screen 36 .
  • the first PROX layer 12 communicates with the second mixing chamber 46 through eight outflow ports 38 formed in the side surface of the eighth cylinder 68 .
  • the second mixing chamber 46 communicates with the second air supply port 30 , and then to a chamber 45 , formed between the seventh and eighth cylinders 67 and 68 , through one second inlet port 39 formed in the side surface of the eighth cylinder 68 .
  • the chamber 45 is formed in the circumferential direction, and communicates with the second PROX layer 13 through eight second inflow ports 49 formed in a screen 47 .
  • the second PROX layer 13 communicates with the reformed gas outlet port 28 through eight second discharge ports 55 formed in the side surface of the eighth cylinder 68 .
  • the number of discharge ports 33 and the like is not limited to eight.
  • the diameters of the discharge ports 33 and the like can be changed in accordance with the distance from the hole 35 and the like, so a uniform amount of gas flows into the first mixing chamber 42 even if a pressure difference exists in it.
  • the discharge ports 33 need not be holes but can be metal mesh-like members.
  • the hole 35 and the like need not be one hole, but can be a plurality of small holes, and the gas may form a swirling flow or may be injected in an oblique direction in order to promote mixing.
  • the reformed gas outlet port 28 is connected to the fuel gas supply port of, e.g., a solid-state polymer-type fuel cell (not shown).
  • the reformed gas (fuel gas) obtained from the reformed gas outlet port 28 and containing a predetermined concentration of hydrogen is supplied to the fuel pole 3 a of the solid-state polymer-type fuel cell 3 , so that power generation is performed.
  • the OFF gas from the fuel pole of a solid-state electrolytic fuel cell 3 may be used as a gas to be combusted by the burner 18 .
  • a cooling flow path 57 with an interior helically formed by round rods 83 is provided downstream from the second mixing chamber 46 .
  • Combustion air inflow and outflow ports 59 a , 59 b are connected to the cooling flow path 57 .
  • Combustion air enters through the inflow port 59 a and flows out through the outflow port 59 b . Hence, the in-flow combustion air is heated and the second PROX layer 13 is cooled.
  • reforming water is supplied through the water supply port 20 , and the burner 18 is ignited to heat the interior of the reformer 2 .
  • the interior of the reformer 2 is heated by the burner 18 , radiation heat of the flame heats the heat transfer partition wall 14 .
  • the combusted exhaust gas passes between the heat transfer partition wall 14 and first cylinder 61 and is exhausted through the combusted exhaust gas outlet port 24 .
  • the inlet portion for the raw material gas to the reforming catalyst layer 8 , the reforming catalyst layer 8 , the pre-heat layer 51 a , and the water heating channel 34 are heated from the inside.
  • the supplied water After being heated to a predetermined temperature, the supplied water passes through the connecting pipe 25 and is mixed with the raw material gas supplied through the raw material gas supply port 26 .
  • the mixture flows through the heating channel 48 downward and reverses its direction at the lower portion to flow upward.
  • the raw material gas is hydrocarbon-based fuel such as city gas.
  • the raw material gas is supplied through the supply port 26 , it passes through the heating channel 48 between the fifth and seventh cylinders 65 and 67 together with the steam and is sent to the pre-heat layer 51 a .
  • the steam and raw material gas heat the shift layer 10 and PROX layer 12 .
  • the raw material gas When the raw material gas enters the pre-heat layer 51 a , as the packing that is packed in the pre-heat layer 51 a is heated by heat from the burner 18 , the raw material gas absorbs this heat and is heated to a predetermined temperature, necessary for the reforming reaction, or more, and enters the reforming catalyst layer 8 . At that time, as is clearly understood, the raw material gas mixed with steam is allowed to flow within the first gas flow path section 51 in the direction from the uppermost side of the pre-heat layer 51 a to the lowest side of the reforming catalyst layer 8 which is in reverse to the flowing direction of the combustion gas within the exhaust flow path 80 .
  • the temperature of the pre-heat layer 51 a near its inlet port can be suppressed low.
  • the raw material gas entering the reforming catalyst layer 8 is, e.g., methane gas, it is reformed by the following reaction: CH 4 +H 2 O ⁇ CO+3H 2
  • reaction proceeds while the reforming catalyst layer 8 absorbs the combustion heat of the burner 18 . More specifically, when the combusted exhaust gas of the burner 18 passes through the exhaust flow path 80 between the heat transfer partition wall 14 and reforming catalyst layer 8 , heat of the combusted exhaust gas is absorbed by the reforming catalyst layer 8 , and a reforming reaction takes place in the reforming catalyst layer 8 while accompanying temperature increase. When the reaction almost reaches an equilibrium, the reformed gas is released from the lower portion of the reforming catalyst layer 8 , reverses its direction at the lower end, and enters the second gas flow path 50 .
  • the round rods 81 are helically formed in the second gas flow path section 50 and the reformed gas rises helically; they perform heat exchange with the reforming catalyst layer 8 as there is no temperature difference in the circumferential direction.
  • the upper end of the second gas flow path section 50 is in contact with the pre-heat layer 51 a where the raw material gas and steam with comparatively low temperatures enter.
  • the temperature of the gas is further decreased, so the gas is released from the upper portion of the second gas flow path section 50 at a temperature appropriate for the CO modifying reaction, is reversed in its direction, and enters the shift layer 10 .
  • the CO modifying reaction of the shift layer 10 is an exothermic reaction
  • the heating channel 48 is formed outside the shift layer 10 .
  • the temperature-increased reformed gas is cooled to reach a temperature appropriate for the selective oxidation reaction.
  • the reformed gas released from the lower portion of the shift layer 10 is reversed in its direction at the lower end and enters the first mixing chamber 42 .
  • the reformed gas is mixed with air supplied through the first air supply port 32 , and while passing through the inlet port 35 is further mixed by the orifice effect of the inlet port 35 , so that a CO selective reaction is performed by the PROX catalyst layer of the first PROX layer 12 .
  • the gas flows into the second mixing chamber 46 through the second inlet port 39 formed in the circumferential portion of the eighth cylinder 68 , and is mixed with air supplied through the air supply port 30 . While further passing through the second inlet port 39 , the gas and air are further mixed by the orifice effect of the second inlet port 39 , and the second CO selective reaction is performed by the PROX catalyst layer of the second PROX layer 13 .
  • the first mixing chamber 42 is provided at the preceding stage. A minimum necessary amount of oxygen is supplied to the reformed gas so as to cause CO oxidation reaction selectively while causing reaction at a plurality of stages, e.g., in the first and second PROX layers 12 and 13 .
  • the heating channel 48 is formed between the shift layer 10 and PROX layer 12 , at the start-up operation, the time taken until a temperature necessary for the reaction is obtained from the heat of the steam is shortened.
  • the respective adjustment valves (not shown) are gradually opened, and water and the raw material gas are supplied through the supply ports 20 and 26 . Then, water is heated by the water heating channel 34 , and is evaporated in the heating channel 48 as it absorbs the reaction heat of the shift layer 10 and PROX layer 12 . Therefore, the temperatures of the shift layer 10 and PROX layer 12 that undergo exothermic reaction to increase their temperatures are suppressed, and can be maintained at a predetermined value by the heat of vaporization of water.
  • the fuel for the burner 18 can be reduced, so that the fuel necessary for generating steam by heating can be economized.
  • the raw material gas, together with the steam heated by the heating channel 48 enters the reforming catalyst layer 8 through the pre-heat layer 51 a.
  • the interior of the pre-heat layer 51 a has already been heated by the burner 18 , and the raw material gas and steam are further heated by the pre-heat layer 51 a .
  • a pre-heater or the like need not be separately provided in order to increase the temperature of the raw material gas to a value necessary for the reforming catalyst layer 8 , so the heat efficiency can be improved.
  • the temperature near the inlet port of the pre-heat layer 51 a for example, the temperature of the outlet port of the flow path section 50 , can be decreased, and the shift layer 10 where a reaction is to take place at a temperature lower than the reaction temperature of the reforming catalyst layer 8 can communicate with the reforming catalyst layer 8 through the second gas flow path section 50 .
  • the raw material gas heated by the pre-heat layer 51 a is subjected to the reforming reaction as it is further heated by the reforming catalyst layer 8 , and flows out from the lower portion of the reforming catalyst layer 8 .
  • the reformed gas with a comparatively high temperature which has flowed out from the lower portion of the reforming catalyst layer 8 rises helically through the second gas flow path section 50 , and is cooled down as it performs uniform heat exchange with the reforming catalyst layer 8 . In other words, while the reformed gas rises swirling through the second gas flow path section 50 , its heat is absorbed, and the temperature drops.
  • the pre-heat layer 51 a is formed at the preceding stage of the reforming catalyst layer 8 , and the inlet port of the pre-heat layer 51 a and the outlet port of the second gas flow path section 50 are formed close to each other, the non-pre-heated raw material gas is introduced to the pre-heat layer 51 a , so that an increase in the temperature of the pre-heat layer 51 a and accordingly in the temperature of the outlet port of the second gas flow path section 50 is suppressed.
  • the shift layer 10 can be formed continuously for the first time.
  • the reformed gas cooled by the second gas flow path section 50 down to a value suitable for the CO modifying reaction enters the shift layer 10 through its upper portion, and CO contained in the reformed gas is modified into carbon dioxide. Although this reaction is an exothermic reaction, the reformed gas is cooled, by heat exchange with the heating channel 48 , down to a value suitable for the CO selective oxidation reaction, and then enters the subsequent PROX layer 12 . At this stage, the reformed gas contains about 0.5% of CO.
  • the insulator 53 is packed in the gap between the second gas flow path section 50 and shift layer 10 .
  • the insulator 53 blocks heat of the second gas flow path section 50 .
  • heat of the second gas flow path section 50 is not directly transferred to heat the shift layer 10 , and the temperature of the shift layer 10 can be held at the predetermined value.
  • the heating channel 48 formed around the shift layer 10 vaporizes the humid steam.
  • This state is equivalent to integrally incorporating a boiler in the reformer 2 .
  • Heat loss of the combusted exhaust gas by the burner 18 can be reduced, and the shift layer 10 and first PROX layer 12 can be cooled by evaporation heat so that they can be suppressed to predetermined temperatures. Therefore, the degree of conversion of CO can be increased in the shift layer 10 , and a methanation reaction and inverse shift reaction, which are undesirable side reactions, can be suppressed in the first PROX layer 12 . Since the reaction heat and sensible heat of the shift layer 10 and first PROX layer 12 can be absorbed in this manner, the heat efficiency can be improved.
  • combustion air, gas or liquid reforming water, raw material gas or the like, or a combination of a plurality of members of them may be utilized as the cooling fluid.
  • combustion air gas or liquid reforming water, raw material gas or the like, or a combination of a plurality of members of them
  • the heating channel 48 may be used as the flow path exclusively for the combustion air, or the flow path of the heating channel 48 may be divided to flow combustion air.
  • the reforming water, raw material gas and the like may be introduced into the reformer 2 by forming flow paths separately from such combustion air flow path.
  • the cooling fluid inflow nozzle can serve also as the raw material gas inflow nozzle. Since the cooling fluid outflow nozzle is not necessary, the arrangement can be simplified.
  • the amount of steam to be supplied into the heating channel 48 is adjusted, the quantity of cooling heat in the heating channel 48 can be changed, and the temperatures of the shift layer 10 , first PROX layer 12 and the like which are important in the reaction can be held at predetermined values.
  • the reformed gas released from the shift layer 10 enters the second and first mixing chambers 46 and 42 where it is to be mixed with air from the air supply ports 30 and 32 . Since the reformed gas is mixed with air while passing through the first mixing chamber 42 and the like, it can be agitated sufficiently if a separate agitator or the like is not provided, and enters the PROX catalyst layer as it is agitated. Therefore, unnecessary hydrogen loss caused by local occurrence of a high oxygen concentration can be prevented in the reaction of the PROX catalyst layer. Since the diameter of the inlet port 35 and the like can be arbitrarily set, the reformed gas can be agitated sufficiently, so that hydrogen loss caused by excessive air can be suppressed.
  • the reformed gas is taken out from the reformed gas outlet port 28 as a gas containing, e.g., 75% of hydrogen, 5% of methane, 19% of carbon dioxide, 1% of nitrogen, and 10 ppm or less of carbon monoxide. Since the reformed gas has a concentration of carbon monoxide of 10 ppm or less in this manner, it can be supplied to a solid-state polymer-type fuel cell, so that it can be used as a fuel gas for the solid-state polymer-type fuel cell.
  • the reformed gas passing through the shift layer 10 reliably merges with air, and since the inlet port 35 and the like are formed at only one portion, when the reformed gas passes through the inlet port 35 and the like, it is mixed with air very well. Since the reformed gas is agitated with air sufficiently in this manner and is introduced to the first PROX layer 12 and the like, the selective oxidation reaction is performed efficiently, and the consumption amount of hydrogen in the selective oxidation reaction can be minimized, so that the CO concentration can be decreased to a predetermined value or less.
  • the shift layer 10 (second shift layer) is provided under the first PROX layer 12 .
  • the shift layer 10 need not be provided under the first PROX layer 12 .
  • the discharge ports 33 and the like are formed at eight portions almost equidistantly in the circumferential direction, and the inlet port 35 and the like are formed at one portion.
  • the present invention is not limited to this arrangement, and a plurality of inlet ports may be formed when necessary.
  • the fins 9 , round rods 81 and the like need not be continuous in the longitudinal direction of the reformer 2 . If the fins 9 , round rods 81 and the like are appropriately divided into a plurality of groups, the thermal stress can be coped with better.

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  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Organic Chemistry (AREA)
  • Engineering & Computer Science (AREA)
  • Combustion & Propulsion (AREA)
  • Inorganic Chemistry (AREA)
  • Health & Medical Sciences (AREA)
  • General Health & Medical Sciences (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Manufacturing & Machinery (AREA)
  • Sustainable Development (AREA)
  • Sustainable Energy (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Hydrogen, Water And Hydrids (AREA)
  • Fuel Cell (AREA)
  • Manufacture, Treatment Of Glass Fibers (AREA)
  • Devices And Processes Conducted In The Presence Of Fluids And Solid Particles (AREA)
US09/969,718 2000-10-10 2001-10-01 Single-pipe cylinder-type reformer Expired - Lifetime US7037472B2 (en)

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AT (1) ATE286850T1 (fr)
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US20060222578A1 (en) * 2005-03-10 2006-10-05 Peter Veenstra Method of starting up a direct heating system for the flameless combustion of fuel and direct heating of a process fluid
US20080090112A1 (en) * 2006-10-13 2008-04-17 Samsung Sdi Co., Ltd. Hydrogen generator and method of operating the same
US20080274021A1 (en) * 2007-05-01 2008-11-06 Jacobus Neels Compact Fuel Processor
US20090053660A1 (en) * 2007-07-20 2009-02-26 Thomas Mikus Flameless combustion heater
US20090056696A1 (en) * 2007-07-20 2009-03-05 Abdul Wahid Munshi Flameless combustion heater
US20090253005A1 (en) * 2004-12-22 2009-10-08 Webasto Ag Reformer for a fuel cell
US20100227235A1 (en) * 2007-05-16 2010-09-09 Nippon Oil Corporation Reformer and indirect internal reforming high temperature fuel cell
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US20090253005A1 (en) * 2004-12-22 2009-10-08 Webasto Ag Reformer for a fuel cell
US8016589B2 (en) 2005-03-10 2011-09-13 Shell Oil Company Method of starting up a direct heating system for the flameless combustion of fuel and direct heating of a process fluid
US20060222578A1 (en) * 2005-03-10 2006-10-05 Peter Veenstra Method of starting up a direct heating system for the flameless combustion of fuel and direct heating of a process fluid
US7704070B2 (en) * 2005-03-10 2010-04-27 Shell Oil Company Heat transfer system for the combustion of a fuel heating of a process fluid and a process that uses same
US20060210468A1 (en) * 2005-03-10 2006-09-21 Peter Veenstra Heat transfer system for the combustion of a fuel and heating of a process fluid and a process that uses same
US20080090112A1 (en) * 2006-10-13 2008-04-17 Samsung Sdi Co., Ltd. Hydrogen generator and method of operating the same
US8114173B2 (en) * 2006-10-13 2012-02-14 Samsung Sdi Co., Ltd. Hydrogen generator and method of operating the same
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US20090056696A1 (en) * 2007-07-20 2009-03-05 Abdul Wahid Munshi Flameless combustion heater
US20090053660A1 (en) * 2007-07-20 2009-02-26 Thomas Mikus Flameless combustion heater
US20150303502A1 (en) * 2012-12-17 2015-10-22 Panasonic Intellectual Property Management Management Co., Ltd. Hydrogen generator
US20160236166A1 (en) * 2015-02-16 2016-08-18 Korea Gas Corporation Fuel processor
US9839898B2 (en) * 2015-02-16 2017-12-12 Korea Gas Corporation Fuel processor
US10128518B2 (en) 2017-04-17 2018-11-13 Honeywell International Inc. Hydrogen production system and methods of producing the same
US10369540B2 (en) 2017-04-17 2019-08-06 Honeywell International Inc. Cell structures for use in heat exchangers, and methods of producing the same

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CA2357960C (fr) 2007-01-30
DE60108329T2 (de) 2006-01-05
EP1197261A3 (fr) 2002-10-16
ATE286850T1 (de) 2005-01-15
DE60108329D1 (de) 2005-02-17
CA2357960A1 (fr) 2002-04-10
AU775034B2 (en) 2004-07-15
US20020042035A1 (en) 2002-04-11
EP1197261B1 (fr) 2005-01-12
AU7821301A (en) 2002-04-11
DK1197261T3 (da) 2005-05-17
EP1197261A2 (fr) 2002-04-17

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